Publication date: 15th May 2025
Post-synthetic transformation of metal chalcogenide nanoparticles is a important route toward rational design of nanoheterostructure; while exchanges altering the cationic component are well established, alteration of the anionic component is less frequently implemented and more poorly understood. We have developed two routes for transforming copper sulfide nanorods into solid-solutions of copper sulfide and copper telluride via anion exchange.[1] One employs a Se/1-octadecene solution and another directly employs dialkyl diselenide molecules. Both are marked by retention of the rod morphology and the hcp anion sublattice to form a metastable wurtzite phase. To better understand the driving force for Se anion exchange in these systems and increase Se incorporation, we have systematically examined the role of various diorganyl diselenides, solvents, and injection suspensions. Thermal decomposition studies coupled with molecular dynamics explain why dialkyl diselenides induce Se anion exchange, but diaryl diselenides do not. Dialkyl diselenides decompose into H2Se, which can directs drive Se anion exchange. A mixture of dialkyl diselenides and dialkyl selenides produced by the reaction of Se and 1-octadecene promotes the greatest incorporation of Se into Cu2-x(S,Se). The presence of thiols impedes the reaction and suggests that formation of alkylthiols may be the driving force for removal of S.
This work was done with the help of Franklin & Marshall College students Kezia Almonte, Kiran Bedi, Michael Boleylchuk, Jiwoo Choi, Nikhita Kuntipuram, Ella Paul, Emily Sandoval-Arteaga, Benjamin Schmidt, and Megna Topiwala, as well as our collaborators at Pennsylvania State University, Adri van Duin and Malgorzata Kowalik. This work was supported by the National Science Foundation through awards DMR-2312618, OAC-192519 (F&M computational cluster), CHE-2320384 (NMR), EAR-0923224 (XRD), and CHE-1724948 (TEM); Research Corporation for the Advancement of Science (CS-PBP-2022-014); the Pennsylvania State University through the Materials Characterization Laboratory and the NSF 2DCC-MIP through cooperative agreements DMR-1539916 and DMR-2039351; and Franklin & Marshall College.
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